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Detection of a plasmon-polariton quantum wave packet

Nature Physics volume 19, pages 656–662 (2023)Cite this article

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Abstract

Plasmon polaritons (plasmons, for simplicity) have become paramount for tailored nanoscale light–matter interaction, and extensive research has been conducted to monitor1,2 and manipulate their spatial3 and spatio-temporal dynamics4. These dynamics result from the superposition of various plasmon modes, which are classical wave packets. Beyond this classical picture, plasmon modes are treated as quasiparticles5,6 and they are considered essential for the realization of future nanoscale quantum functionality7,8,9,10. Implementing and demonstrating such functionality requires access to the quasiparticle’s quantum state to monitor and manipulate its corresponding quantum wave packet dynamics in Hilbert space. Here we report the local detection of nanoscale plasmon quantum wave packets using plasmon-assisted electron emission as a signal in coherent two-dimensional nanoscopy11. The observation of a quantum coherence oscillating at the third harmonic of the plasmon frequency is traced back to the superposition of energetically non-adjacent plasmon occupation number states and is therefore a direct fingerprint of the quantum wave packet. Beyond demonstrating the existence of a plasmon quantum wave packet via the coherence between certain occupation number states and providing an improved model for plasmon-assisted electron emission processes, the results may enable time-dependent probing and manipulation of coupled quantum states and dynamics on the nanoscale.

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Fig. 1: Quantum model of plasmon-polariton-assisted multi-quantum electron emission from a plasmonic resonator probed by 2D nanoscopy.
Fig. 2: Comparison of measured and simulated rephasing 2D spectra of plasmon-polariton-assisted multi-quantum electron emission.
Fig. 3: Impact of 3ωpp quantum coherences of the plasmon polariton on the rephasing 2D spectrum.

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Data availability

Data that support the plots within this paper and other findings of this study are available from the corresponding author upon reasonable request. Source data are provided with this paper.

Code availability

The codes that support the findings of this study are available from the corresponding author upon reasonable request.

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Acknowledgements

We gratefully acknowledge funding by the European Research Council (ERC consolidator grant ‘MULTISCOPE’ – 614623) (T.B.) and the Deutsche Forschungsgemeinschaft (423942615 to T.B. and 410519108 to W.P.). We thank P. Malý for fruitful discussions, ELMITEC Elektronenmikroskopie GmbH for technical PEEM support, the Rechenzentrum of the University of Würzburg for providing computational resources and our mechanical and electronics workshop as well as technical staff of the Institut für Physikalische and Theoretische Chemie, Würzburg, for special support in the realization of the experimental set-up.

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Authors and Affiliations

  1. Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Am Hubland, Würzburg, Germany

    Sebastian Pres, Bernhard Huber, Matthias Hensen, Daniel Fersch, Victor Lisinetskii & Tobias Brixner

  2. Nano-Optics and Biophotonics Group, Experimental Physics 5, University of Würzburg, Am Hubland, Würzburg, Germany

    Enno Schatz, Daniel Friedrich & Bert Hecht

  3. Fakultät für Physik, Universität Bielefeld, Universitätsstr. 25, Bielefeld, Germany

    Ruben Pompe & Walter Pfeiffer

  4. Center for Nanosystems Chemistry (CNC), Universität Würzburg, Theodor-Boveri-Weg, Würzburg, Germany

    Tobias Brixner

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Contributions

T.B., B. Hecht and M.H. initiated and supervised the experiments. D. Friedrich and E.S. performed the fabrication of the plasmonic nanoslit resonators and the SEM measurements. V.L. adjusted and maintained the NOPA system. D. Fersch, M.H., B. Huber and S.P. planned and executed the 2D nanoscopy experiments. S.P. performed the pulse characterization and reconstruction. M.H., W.P., R.P. and S.P. developed the theoretical model. S.P. implemented and executed the FDTD simulations and the quantum dynamical simulations. S.P. wrote the manuscript with input from all co-authors. All authors contributed to the discussion and have given approval to the final version of the manuscript.

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Correspondence to Bert Hecht, Walter Pfeiffer or Tobias Brixner.

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Pres, S., Huber, B., Hensen, M. et al. Detection of a plasmon-polariton quantum wave packet. Nat. Phys. 19, 656–662 (2023). https://doi.org/10.1038/s41567-022-01912-5

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